A novel radical gold dithiolene complex exhibits a hexagonal columnar mesophase, as confirmed by optical microscopy, DSC analysis and X-ray diffraction. The extent of delocalization of the spin density in such a complex was analyzed by EPR. Temperature dependent magnetization measurements reveal that the global magnetic moment is remarkably affected at the liquid-crystalline phase transition with a marked hysteresis signature, rare behavior among the few described paramagnetic discotic phases. In addition, these molecules were found to strongly aggregate in solution into one-dimensional fibers with a mean diameter of 60 nm extending over micrometres, leading to the formation of gel-like structures. These fibers are stable and can be isolated on surfaces. The gelation of the system can also be detected by temperature-dependent magnetic measurements.
Self‐assembling features, chiroptical activity, and spin filtering properties are reported for 2,15‐ and 4,13‐disubstituted [6]helicenes decorated in their periphery with 3,4,5‐tris(dodecyloxy)‐N‐(4‐ethynylphenyl)benzamide moieties. The weak non‐covalent interaction between these units conditions the corresponding circularly polarized luminescence and spin polarization. The self‐assembly is overall weak for these [6]helicene derivatives that, despite the formation of H‐bonding interactions between the amide groups present in the peripheral moieties, shows very similar chiroptical properties both in the monomeric or aggregated states. This effect could be explained by considering the steric effect that these groups could generate in the growing of the corresponding aggregate formed. Importantly, the self‐assembling features also condition chiral induced spin selectivity (CISS effect), with experimental spin polarization (SP) values found between 35–40 % for both systems, as measured by magnetic‐conducting atomic force microscopy (AFM) technique.